SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Cailiang Yue,Yukun Tian,Linlin Zhu,Nan Sun,Zhiqi Zhou,Fuqiang Liu,Yifei Sun
Photocatalytic 1 O 2 generation has emerged as a promising technology for environmental remediation and organics synthesis. Nevertheless, the efficiency of photocatalytic 1 O 2 generation via O 2 activation through charge-transfer mechanism remains challenging in carbon nitride due to the weak dielectric screening effect. Herein, series of uric acid (UA)-modified ultrathin carbon nitride nanosheets (UCN-x) were fabricated by the simple supramolecular self-assembly process. Comprehensive characterizations revealed that the incorporation of UA pigment would induce purine structure into heptazine skeleton. Photocatalytic experiments showed that the modification of UA greatly enhanced photocatalytic 1 O 2 generation ability. The optimal UCN-2 exhibited superior photocatalytic degradation of tetracycline (TC) with the normalized TC degradation rate up to 10.03 mg TC g cat −1 min −1 , which was 2.1–31.1 times as high as that of reported photocatalysts. What's more, UCN-2 exhibited excellent photocatalytic TC degradation across diverse aqueous conditions, demonstrating significant potential in environmental remediation. Time-dependent density functional theory (TD-DFT) calculation revealed that the doping of UA could trigger the spatial separation of h + /e − distribution, with h + concentrated in UA pigment and e − concentrated in adjacent heptazine ring. The engineered adjacent redox sites were precisely tailored to align with the charge-transfer mechanism for photocatalytic 1 O 2 generation. This work established a fundamental framework for designing highly efficient photocatalysts with manipulated O 2 activation.
研究领域:
环境科学
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材料化学
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光催化
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纳米材料
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环境修复
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Yixi Wang,Wenqing Xu,Zhi Liu,Yulong Shan,Wanrong Chen,Xinyu Zhang,Tingyu Zhu
Controlling both CO and NOx pollutants without additional cost is necessary but challenging, especially in industrial flue gas with complex components. Previous studies mainly focused on the effect of O 2 and SO 2 on the CO oxidation side reaction and valence state of Ir species on various catalysts, while neglecting the impact on NO conversion pathway. Herein, we propose an "ineffective reaction pathway" in the presence of O 2 with nitrate as an intermediate according to the results of in situ DRIFTS and DFT. And we also reveal the contribution of SO 2 in inhibiting the adsorption of O 2 and promoting the selective adsorption of NO and CO even at lower injection concentrations, based on the oxidation of SO 2 on Ir(111). This is quite a favorable characteristic for the treatment of industrial flue gas, resolving the long–standing dispute on the involvement of these components in the CO–SCR reaction. Under specific conditions (CO/NO=20, O 2 =5%, SO 2 =200 ppm) at 250 °C, the NOx conversion is as high as 78%. These results will contribute to the development of more efficient catalysts in the future for simultaneously controlling two pollutants (CO and NOx).
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
Science Bulletin
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2025
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IF 21.1
Ergui Luo,Jingyi Liang,Kexuan Zhang,Xian Wang,Luozhen Jiang,Tianjun Hu,Junming Zhang,Junjie Ge,Jianfeng Jia
Electrochemical two-electron oxygen reduction reaction (2e − ORR) serves as an appealing approach for green hydrogen peroxide (H 2 O 2 ) production. However, the corresponding progress in efficient non-precious metal catalysts for acidic 2e − ORR has not kept pace, with the research model being almost confined to Co-based system. Here, guided by molecular dynamics simulations, the active nature and origin of pyrolyzed Cr−N 4 catalysts for ORR are unveiled, wherein the over-strong oxygen affinity of the Cr center is counterbalanced by a spontaneous axial O-coordination. By creating an oxidation-induced electron-deficient environment, the Cr−N 4 can be flexibly tailored for selective H 2 O 2 formation. A single-atom Cr−N 4 /C(O) catalyst is developed experimentally, which rivals and even slightly outperforms its Co-based counterpart in terms of selectivity (92% versus 71%) and productivity (202 versus 145 mmol g cat −1 h −1 ) for H 2 O 2 . More encouragingly, the Cr-based catalysts exhibit minimal reactivity towards H 2 O 2 -related side reactions, with the metal component being robust against leaching. This research marks the first identification of pyrolyzed Cr−N 4 catalysts as competent for acidic two-electron O 2 reduction to H 2 O 2 . The innovative models and insights offer profound guidance for the design of future-generation catalysts for electrochemical H 2 O 2 synthesis.
研究领域:
电催化
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材料科学
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能源化学
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可持续化学
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计算化学
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产品关联
DOI
PubMed
高影响因子
Energy Materials
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2025
·Vol. 5
·期 11
·N
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IF 11.2
Shukai Liu,Huang Tan,Gaole Dai,Shiyun Xiong,Yu Zhao,Benxia Li
The oxygen evolution reaction (OER), as a pivotal process in electrochemical water splitting, directly determines energy conversion efficiency. Ruthenium (Ru)-based catalysts have gained considerable attention in recent years due to their decent intrinsic activity in acidic media. Previous studies have demonstrated that while Ru exhibits superior OER activity compared to RuO2 in acidic environments, its operational stability remains markedly inferior. This performance dichotomy, coupled with the persistent challenges of active species dissolution and catalyst particle aggregation during prolonged operation, significantly hinders their practical implementation in electrochemical systems. To address these challenges, this study develops a carbon nanotube (CNT)/Fe-Ni@RuO2@PANI-350 composite catalyst composed of RuO2 nanoparticles supported on bimetallic Fe-Ni modified CNTs (CNT/Fe-Ni) and encapsulated with polyaniline (PANI). This catalyst utilizes the anchoring effect of bimetallic Fe-Ni sites and the spatial confinement effect of PANI coating layer, effectively inhibiting the dissolution and agglomeration of RuO2 during both high-temperature processing and electrochemical operation, thereby significantly enhancing electrochemical stability. The anchoring strength of RuO2 nanoparticles on CNT/Fe-Ni support via the nano-confinement effect, as well as the microscopic mechanisms underlying the performance enhancement, are revealed by density functional theory calculations and experimental characterizations. The composite catalyst demonstrates fascinating OER performance in 0.5 M H2SO4, exhibiting a low Tafel slope of 39.1 mV dec-1 as well as low overpotentials of 188 and 225 mV at current densities of 10 and 100 mA cm-2, respectively. Remarkably, the composite catalyst demonstrates significantly enhanced stability, exhibiting only ~30 mV overpotential increase during 150 h continuous operation at 10 mA cm-2. This study highlights a simple yet effective nano-confinement strategy to address the challenges of Ru-based catalysts, and provides a practical paradigm for designing and preparing highly efficient OER electrocatalysts with enhanced stability.
研究领域:
电化学
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催化
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纳米材料
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能量转换
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Yu Luo,Chenchen Liu,Jiahui Liu,Xueming Liu,Yang Zhou,Xinwen Ou,Bo Weng,Jin Jiang,Bin Han
Photocatalytic O 2 reduction presents a sustainable strategy for H 2 O 2 synthesis, while the in-situ decomposition of H 2 O 2 significantly deteriorates the activity and stability. Here, by introducing anthraquinone centers into covalent organic frameworks (DQTb-COFs), for the first time, we realized the suppression of in-site decomposition of generated H 2 O 2 via site-engineering of COFs. Under visible light irradiation, DQTb-COFs achieves an H 2 O 2 generation rate of 1844.1 μmol h −1 g −1 without sacrificial agents, which is about 3.4 times that of its counterpart without anthraquinone centers (DATb-COFs). The generated H 2 O 2 on DATb-COFs is readily reduced into hydroxyl radicals (•OH), which is not observable on DQTb-COFs. Experiments and calculations demonstrated that the anthraquinone centers of DQTb-COFs can enhance the generation of H 2 O 2 by facilitating the utilization of O 2 and promoting the desorption of H 2 O 2 . This work highlights how to inhibit the in-situ decomposition of H 2 O 2 via site-engineering of COFs, and blazes a new trail for highly efficient H 2 O 2 photosynthesis.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
PROCEEDINGS OF THE COMBUSTION INSTITUTE
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2024
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IF 5.3
Nan Liu,Qi Chen,Xianwu Jiang,Jie Chen,Lidong Zhang,Jiaying Pan,Haiqiao Wei,Xingqian Mao
This work presents a three-stage hybrid nanosecond discharge (NSD) and direct current (DC) discharge assisted n -C 5 H 12 /O 2 /N 2 ignition with lower discharge energy and higher energy efficiency. The reaction rate coefficients between O 2 (a 1 Δ g ) and n -C 5 H 12 are updated by mass/Master equation simulation. The promotive ignition enhancement via reaction channel O 2 (a 1 Δ g ) + n -C 5 H 12 → C 5 H 10 + H 2 O 2 in the hybrid NSD/DC discharge is demonstrated. The results show that the ignition delay time of the three-stage hybrid plasma assisted ignition is 1–2 orders of magnitude shorter than that of the two-stage hybrid discharge when the reduced electric field strength in the DC discharge stage is over 10 Td. Meanwhile, the plasma-enhanced energy efficiency of three-stage hybrid discharge increases. This improved efficiency on ignition enhancement is due to the kinetic enhancement by the electronically excited species and radicals (O 2 (a 1 Δ g ), O( 1 D), N 2 (B) and O). The kinetic and thermal effects by plasma are effectively intergated to enhance ignition. However, more discharge energy deposited in the vibrationally excited states N 2 ( v ) in the two-stage hybrid discharge is less efficient on ignition enhancement due to the thermal contribution via vibrational-translational relaxation. In the aspect of NO x /N 2 O emissions, reduction efficiency of the three-stage hybrid discharge is two times higher than that of the two-stage hybrid discharge. By controlling the N/N( 2 D) production pathway e + N 2 → e + N + N( 2 D), the three-stage hybrid discharge reduces NO x and N 2 O production by 61.1 % and 90 %, respectively. The results show that the ignition delay time is non-monotonically dependent on the discharge pulse number. There exist optimal pulse number, reduced electric field and effective threshold power density of DC discharge to achieve maximum ignition enhancement and low NO x /N 2 O emissions. This study provides valuable insights into the use of NSD/DC hybrid discharge technology in advanced engines to achieve energy-efficient ignition enhancement and reduce NO x /N 2 O emissions.
研究领域:
能源科学
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环境科学
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化学动力学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS TODAY
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2024
·
IF 5.2
Jipeng Wang,Xinli Tong,Chen Guo,Yahui Wei
The high entropy oxides are widely studied as the potential catalytic materials owing to their unique structure and excellent properties. In this work, a new high entropy oxide catalyst MnFeCoNiCuO x was successfully prepared and used for the oxidative condensation reaction of furfural (FUR) and aliphatic alcohol , where the carbon-chain length can be selectively increased under the mild conditions. For the selective oxidative transformation of FUR with n-butanol, a more than 99.0 % conversion of FUR and 91.5 % selectivity of 2-(furanyl-2-methylene) butanal was obtained at 80 ºC for 2 h. In addition, the oxidative condensation of FUR with ethanol, n-propanol, n-pentanol, n-hexanol and n-heptanol was also carried out with the MnFeCoNiCuO x - LiOH as catalyst system in the presence of molecular oxygen , where a moderate to high product yields were acquired. Furthermore, the characterizations of catalyst showed that the existence of abundant oxygen vacancy and high specific area was greatly important to the catalytic reactions .
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Yajuan Jiang,Shining Zhang,Chunyu Xu,Bin Jia,Shijie Ren,Wenyu Zheng,Yicong Huang,Kunpeng Jiang,Xiuyun Zhang,Yunyun Zhao,Guisheng Zhu,Huarui Xu
In this paper, biomass carbon@Li(Ni 0.6 Co 0.4 )O 2 (BC@LNCO) micron-tube is successfully synthesized via a bio-templating method as cathodic material for lithium-ion hybrid supercapacitors. Cobalt nickel subcarbonates nanowires arrays are homogeneously grown on bagasse substrate via a unique synthesis strategy using a toluene-water interface reaction process, which subsequently transform as BC@LNCO micron-tube after lithiation process. The distinctive biomass fibre structure of bagasse biomass carbon leads to a significant enhancement in active sites in the BC@LNCO composite, which facilitates lithium-ion diffusion and enhances the contact area between the electrode and electrolyte. So, the prepared BC@LNCO electrode demonstrates improved electrical performances with a high specific capacitance of 921 F g −1 at 1 A g −1 and a good rate performance with 72 % retention at 10 A g −1 . In addition, the lithium-ion hybrid supercapacitor is fabricated with BC@LNCO and activated carbon (AC) as positive and negative electrodes, respectively. The BC@LNCO//AC device demonstrates a good energy density of 56.25 Wh kg −1 at 818.4 W kg −1 , and maintains 25.06 Wh kg −1 when the power density is up to 8143.42 W kg −1 , indicating that the prepared BC@LNCO composite can be a promising candidate as electrode material for Li-ion hybrid supercapacitor.
研究领域:
材料科学
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能源存储
✓ 已验证
产品关联
DOI
高影响因子
Chemical Science
·
2024
·
IF 7.6
Yinglei Tao,Tao Wang,Xingyu Yu,Ke Gong,Hao Gong,Haixia Chen,Xiaoli Fan,Aidi Zhang,Xianli Huang,Kun Chang,Jianping He
Li–O2 batteries (LOBs) boast an exceptionally high theoretical energy density; however, the slow kinetics of the oxygen electrode reaction have been a significant hurdle in their advancement and practical application. In this study, a composite of bismuth oxyhalide heterojunction incorporated with metal–organic frameworks (MOFs) was engineered on carbon cloth (Zr-MOF/BiOIBr/CC) as an efficient bifunctional catalyst to enhance the oxygen electrode reaction in photo-assisted LOBs. Compared to Zr-MOF/CC, Zr-MOF/BiOIBr/CC significantly expands the light absorption spectrum of the catalyst. Furthermore, the built-in electric field in the heterojunction aids in the separation and directional movement of photogenerated carriers, thereby expediting the reaction kinetics of LOBs. Consequently, the photo-assisted LOBs with Zr-MOF/BiOIBr/CC as the cathodes display a discharge potential of 3.05 V, a low charge potential of 3.20 V, and an energy efficiency of up to 95.3%, and can sustain an extended cycle life of over 255 cycles. This study underscores the potential application of MOFs/semiconductor heterostructural materials in photo-assisted LOBs and offers insights into the systematic design of photo-assisted air batteries and other advanced semiconductors.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
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2024
·
IF 5.3
Xiang Yu,Yuwei Mi,Zihan Gong,Yongfang Zhang,Lei Wang,Suyuan Zeng
Constructing heterojunctions is an effective strategy for increasing semiconductor photocatalytic activity. Herein, a Bi2O3/Bi4O5Br2 type-II heterojunction was synthesized using a simple one-pot solvothermal route. The 0-dimensional (0D) Bi2O3 nanoparticles are uniformly distributed within the 2D Bi4O5Br2 nanosheets with (101̅) facets dominantly exposed. In comparison with pure Bi2O3 and Bi4O5Br2, they show higher photocatalytic activity degradation of resorcinol (RO) and Rhodamine B (RhB). The Bi2O3/Bi4O5Br2 composite containing 10% Bi2O3 (BOB4) displays the best photocatalytic activity. For instance, compared with pure Bi4O5Br2 and Bi2O3, the k(RO) values of BOB4 (0.58 h–1) are 3.1 and 4.8 times higher. The enhanced photocatalytic activity is attributed to the formation of a large heterojunction interface that results from the homogeneous distribution of Bi2O3 nanoparticles in the Bi4O5Br2 nanosheet, which effectively enhances the photogenerated charge separation in a type-II mode. Major active species include superoxide radicals (•O2–), hydroxyl radicals (•OH), and holes (h+). In addition, the Bi2O3/Bi4O5Br2 photocatalysts exhibit outstanding resistance to inorganic ions, pH, water matrix, as well as outdoor sunlight and favorable stability and biocompatibility. This work presents a simple method to construct Bi-based heterojunction architectures for photoactivity improvement.
研究领域:
材料科学
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环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Wei Du,Zhihua Zhang,Jundi Wang,Nan Song,Xuezhi Duan,Xinggui Zhou
Propylene epoxidation by H 2 and O 2 to propylene oxide (HOPO), as a novel method for PO production, has attracted widespread attention due to its economic and environmental advantages. Acrolein is a notable byproduct arising in HOPO reaction over Au/TS-1 catalyst, and is traditionally thought to be exclusively formed on Au site through propylene oxidation. However, on the intraporous and external surface Au sites of Au-Ti catalysts, the HOPO reaction have been shown to proceed by different mechanisms, yet the effect of active sites distribution on acrolein formation is far from being understood. Herein, we found that the reaction orders in acrolein formation on Au/TS-1 catalyst (H 2 , 0.19; O 2 , 0.44; C 3 H 6 , 0.44) relative to Au/TS-1 with blocked pores (Au/TS-1-B) catalyst (H 2 , −0.36; O 2 , 0.61; C 3 H 6 , 0.52) were quite different, suggesting a variation in the reaction pathway on the catalysts with different Au locations. Moreover, it is found that PO can be converted to acrolein by O 2 on TS-1 zeolite, which is absent on TS-1-B zeolite without micropores. Consequently, acrolein formation on Au/TS-1 catalyst can proceed through two parallel pathways: propylene hydro-oxidation on Au site, and PO conversion by O 2 inside micropores. Furthermore, by designing and preparing the Au/TS-1 catalysts with different structures, the Au locations are closely related to acrolein formation mechanism and kinetic behaviors. This work provides kinetic insights into the acrolein formation pathways in the HOPO reaction on Au/TS-1 catalyst, and is helpful to the rational design and preparation of efficient catalysts with high selectivity.
研究领域:
催化化学
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材料科学
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环境化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Shan Jiang,Jing Cao,Minna Guo,Dongdong Cao,Xuemei Jia,Haili Lin,Shifu Chen
Elemental red phosphorus (RP) has an ultra-low activity of splitting water for H 2 and O 2 evolution. In this study, RP was decorated by trace amount of WO 3 to greatly enhance the photocarriers separation and photocatalytic activity for overall water splitting under visible light. The 2.5% WO 3 /RP composite achieved the highest activity to produce H 2 and O 2 , and the activity was 7.0 times that of pure RP under visible light (λ ≥ 420 nm). The significantly increased photocarriers separation of WO 3 /RP was ensured by transient photocurrent, electrochemical impendence, photoluminescence, and time-resolved photoluminescence characterizations. More importantly, WO 3 /RP maintained high stability when it was persistently used for 20 cycles. Based on the reactive oxygen species ( O 2 − and OH) detected during the photocatalytic process, an S-scheme mechanism was proposed for WO 3 /RP composites to efficiently separate the photocarriers. This work provides a notion for improving the overall water splitting activity of RP via an S-scheme photocarriers separation mode.
研究领域:
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）